Xu Yi Ning, Li Wenjing, Fu Huai Qin, Zhang Xin Yu, Zhao Jia Yue, Wu Xuefeng, Yuan Hai Yang, Zhu Minghui, Dai Sheng, Liu Peng Fei, Yang Hua Gui
Key Laboratory for Ultrafine Materials of Ministry of Education, Shanghai Engineering Research Center of Hierarchical Nanomaterials, School of Materials Science and Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai, 200237, China.
Centre for Catalysis and Clean Energy, Gold Coast Campus, Griffith University, Gold Coast, QLD 4222, Australia.
Angew Chem Int Ed Engl. 2023 May 2;62(19):e202217296. doi: 10.1002/anie.202217296. Epub 2023 Apr 4.
The electrocatalytic reduction of carbon dioxide provides a feasibility to achieve a carbon-neutral energy cycle. However, there are a number of bottleneck issues to be resolved before industrial application, such as the low conversion efficiency, selectivity and reaction rate, etc. Engineering local environment is a critical way to address these challenges. Here, a monolayer MgAl-LDH was proposed to optimize the local environment of Cu for stimulating industrial-current-density CO -to-C H electroreduction in neutral media. In situ spectroscopic results and theoretical study demonstrated that the Cu electrode modified by MgAl-LDH (MgAl-LDH/Cu) displayed a much higher surface pH value compared to the bare Cu, which could be attributed to the decreased energy barrier for hydrolysis on MgAl-LDH sites with more OH ions on the surface of the electrode. As a result, MgAl-LDH/Cu achieved a C H Faradaic efficiency of 55.1 % at a current density up to 300 mA cm in 1.0 M KHCO electrolyte.
二氧化碳的电催化还原为实现碳中性能源循环提供了可行性。然而，在工业应用之前，仍有许多瓶颈问题需要解决，例如低转化效率、选择性和反应速率等。设计局部环境是应对这些挑战的关键途径。在此，提出了一种单层MgAl-LDH来优化Cu的局部环境，以促进中性介质中工业电流密度下CO₂到C₂H₄的电还原。原位光谱结果和理论研究表明，与裸Cu相比，MgAl-LDH修饰的Cu电极（MgAl-LDH/Cu）表现出更高的表面pH值，这可归因于MgAl-LDH位点上水解的能垒降低，电极表面有更多的OH⁻离子。结果，在1.0 M KHCO₃电解液中，MgAl-LDH/Cu在电流密度高达300 mA cm⁻²时实现了55.1%的C₂H₄法拉第效率。
